We have previously reported on a method for reconstructing quantitative data from 99mTc single photon emission computed tomography (SPECT) images based on corrections derived from X-ray computed tomography, producing accurate results in both experimental and clinical studies. This has been extended for use with the radionuclide 201Tl. Accuracy was evaluated with experimental phantom studies, including corrections for partial volume effects where necessary. The quantitative technique was used to derive standardized uptake values (SUVs) for 201Tl evaluation of brain tumours. A preliminary study was performed on 26 patients using 201Tl SPECT scans to assess residual tumour after surgery and then to monitor response to treatment, with a follow-up time of 18 months. Measures of SUVmax were made following quantitative processing of the data and using a threshold grown volume of interest around the tumour. Phantom studies resulted in the calculation of concentration values consistently within 4% of true values. No continuous relation was found between SUVmax (post-resection) and patient survival. Choosing an SUVmax cut-off of 1.5 demonstrated a difference in survival between the 2 groups of patients after surgery. Patients with an SUVmax <1.5 had a 70% survival rate over the first 10 months, compared with a 47% survival rate for those with SUVmax >1.5. This difference did not achieve significance, most likely due to the small study numbers. By 18 months follow-up this difference had reduced, with corresponding survival rates of 40% and 27%, respectively. Although this study involves only a small cohort, it has succeeded in demonstrating the possibility of an SUV measure for SPECT to help monitor response to treatment of brain tumours and predict survival.